DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 6
·1595-1601
·
IF 4
Ziwei Wang,Lijuan Li,Weijin Wang,Runlin Wang,Guangzhe Li,Hang Bian,Dongxia Zhu,Martin R. Bryce
Cyclometalated Ir(III) complexes as photosensitizers (PSs) have attracted widespread attention because of their good photostability and efficient 1O2 production ability. However, their strong absorption in the UV-vis region severely limits their applications in photodynamic therapy (PDT) because the short wavelength illuminating light can be easily absorbed by the skin and subcutaneous adipose tissue causing damage to the patient's normal tissue. Herein, mono- and tetra-nuclear Ir(III) complex-porphyrin conjugates are rationally designed and synthesized, especially [TPP-4Ir]4+ exhibits obvious aggregation-induced emission (AIE) characteristics. PSs comprising Ir(III) complex-porphyrin conjugates self-assembled as nanoparticles (NPs) are successfully achieved. The obtained [TPP-Ir]+ NPs and [TPP-4Ir]4+ NPs exhibit long wavelength absorption (500–700 nm) and near-infrared emission (635–750 nm), successfully overcoming the inherent defects of short wavelength absorption of traditional Ir(III) complexes. Moreover, [TPP-4Ir]4+ NPs exhibit good biocompatibility, high 1O2 generation ability, low half-maximal inhibitory concentration (IC50) (0.47 × 10−6 M), potent cytotoxicity toward cancer cells and superior cellular uptake under white light irradiation. This work extends the scope for transition metal complex PSs with promising clinical applications.
研究领域:
材料科学
·
纳米技术
·
光动力疗法
·
癌症研究
·
光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2023
·
IF 11.1
Yafei Wang,Chenhao Wang,Shen Yan,Yingchun Li,Chen Cai,Huiling Liu,Peng Ren,Mengmeng Wang,Shaoping Kuang
To reduce the adverse effects of antibiotics and antibiotic resistance genes (ARGs) in the environment, nitrogen-doped biochar (NLBH), derived from lincomycin fermentation dregs (LFD), was employed as an activator in a persulfate (PDS) oxidation system. The system was evaluated for its ability to degrade tetracycline (TC), inactivate antibiotic resistant bacteria (ARB) and remove ARGs. The degradation efficiency of TC in the NLBH/PDS system (70.1%) was higher than that in the pristine biochar/PDS system (10.3%). It was confirmed that the defects and edge pyridinic nitrogen generated in the nitrogen doping process were the reactive sites for PDS activation. According to electron paramagnetic resonance (EPR) and radical quenching experiments, the major mechanism for PDS activation was a non-radical pathway dominated by singlet oxygen ( 1 O 2 ). Radical pathways involving sulfate (SO 4 · - ) and hydroxyl radicals (·OH) were also at play in the NLBH/PDS system, but their role was minor. TC was principally degraded by hydroxylation , demethylation, and decarboxylation , and within 90 min, the NLBH/PDS system effectively inactivated 71.5% of ARB ( Pseudomonas sp. HLS-6). Intracellular ARGs (iARGs; sul 1, sul 2) and intI 1 had log reduction efficiencies of 2.73–4.04 and 2.70, respectively, whereas, extracellular ARGs ( sul 1 and sul 2) and intI 1 accumulated noticeably by 1.52–4.18-and 4.92-log, respectively. This work highlights a promising alternative technique for the removal of antibiotics, ARB and iARGs in future advanced wastewater treatment systems.
研究领域:
环境科学
·
化学工程
·
微生物学
·
废物管理
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Liyuan Wu,Pengpeng Guo,Xin Wang,Haiyan Li,Angzhen Li,Kaiyu Chen
Peroxymonosulfate (PMS) activation methods have attractive advantages in advanced oxidation process (AOPs) due to their powerful ability of directly or indirectly generating various reactive oxygen species (ROS). Herein, trace amount of Fe(III) ions were added into the commercial-CoS 2 /PMS system to improve the CoS 2 /PMS decomposition for organics removal. The organics removal efficiency could reach >90% towards methylene blue (MB), diclofenac sodium (DCF), sulfamethoxazole (SMX) and bisphenol A (BPA) in the CoS 2 /Fe(III)/PMS system, with the kinetic apparent rate constant k obs of 0.141, 0.206, 0.247 and 0.091 min −1 , respectively. The synergistic effect between Fe(III) ions and sulfur-vacancies on CoS 2 for PMS degradation were revealed for the first time in cobalt sulfides/PMS system. Quenching experiments and ESR analysis proved that 1 O 2 was the major ROS and was produced mainly by the hydrolysis of SO 5 • – . Besides, the high degradation efficiency was obtained by the contribution of SO 4 • – and • OH. Electron spin–resonance spectroscopy (ESR), cyclic voltammetry (CV) and Raman spectrum data revealed that the addition of Fe(III) ions could optimize the intensity of sulfur vacancies on the CoS 2 surface, which hindered the PMS reduction ability of Co(II), but accelerated the PMS oxidation to form 1 O 2 . The degradation path of MB was analyzed by liquid chromatograph-mass spectrometer (LC-MS). The mechanism studies speculated that the sulfur vacancies of CoS 2 provided the binding sites for Fe(III) ions with Co(II), which facilitated the PMS activation by Co(III).
研究领域:
环境化学
·
催化
·
水处理
·
高级氧化过程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiayu Xiao,Luo Hai,Ke Yang,Yuze Luo,Zefeng Wang,Junqin Li,Chunlei Ou,Li Wang,Le Deng,Dinggeng He
Reactive oxygen species (ROS) such as hydroxyl radicals ( OH) and singlet oxygen ( 1 O 2 ) have emerged as promising therapeutic agents for combating biofilm-associated bacterial infections. However, the hypoxic microenvironments in the biofilms severely hinder the ROS production. Herein, we have rationally integrated copper peroxide (CP) and indocyanine green (ICG) into a polydopamine (PDA) nanoparticle to construct a versatile hybrid nanoplatform (PDA/CP/ICG), which can enhance ROS generation for highly efficient biofilm elimination by relieving hypoxic microenvironment. When the PDA/CP/ICG accumulates at the infection site or biofilm, the acidic microenvironment triggers the co-release of Cu 2+ and H 2 O 2 , and the former can catalyze the conversion of self-supplied H 2 O 2 into OH via a Fenton-like reaction and consume the overexpressed antioxidant glutathione (GSH) to further promote the oxidative stress. Moreover, with the help of an 808 nm laser, the hyperpyrexia caused by PDA induces the decomposition of CP into O 2 that is immediately converted by ICG into 1 O 2 . The PDA/CP/ICG shows satisfactory antibacterial and antibiofilm effect due to the self-amplified production of OH and 1 O 2 , and outstanding wound healing with good in vivo biosafety. Overall, this study provides a facile paradigm in ROS-based biofilm elimination, and the proposed hypoxia-irrelevant bactericidal nanoplatform has great potential for future biomedical applications.
研究领域:
生物材料
·
纳米医学
·
抗菌治疗
·
生物膜消除
·
伤口愈合
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ran Hao,Gangwan Zhang,Jiahe Zhang,Leyong Zeng
The weak catalytic activity of nanocatalysts and the insufficient endogenous hydrogen peroxide (H 2 O 2 ) in tumor microenvironment (TME) seriously restricted the efficacy of catalytic therapy, and the non-degradability of inorganic nanocarriers was also unfavorable for their clinical applications. Herein, by depositing gold nanoparticles (AuNPs) and platinum nanoparticles (PtNPs) with ultrasmall size and modifying photosensitizer (IR808), a biocompatible bovine serum albumin (BSA) nanoplatform (BSA@Au/Pt-IR808) with triple-amplification of enzyme activity was constructed to enhance photodynamic therapy (PDT) and catalytic therapy. Ultrasmall AuNPs possessed glucose oxidase (GOx)-like activity, by which the self-supplying H 2 O 2 accelerated the dual-enzyme activity of peroxidase (POD) and catalase (CAT) of ultrasmall PtNPs, promoting the generation of hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ). Compared with BSA-IR808 and BSA@Pt, the yields of 1 O 2 and ·OH of BSA@Au/Pt-IR808 increased by 38.2% and 18.6%. Under the combination action of photothermal therapy (PTT)/PDT/catalytic therapy of BSA@Au/Pt-IR808, the cell viability significantly reduced to 12.8%, and the tumors were completely eliminated, demonstrating the enhanced PDT and catalytic therapy against breast cancer.
研究领域:
纳米技术
·
生物医学工程
·
癌症治疗
·
材料科学
·
光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Caihong Liu,Xihui Jiang,Zhiqiang Sun,Rui Gao,Min Wang,Qiang He,Jun Ma
Catalytic membranes that enable simultaneous micropollutant degradation during oil/water separation have emerged as a promising candidate for treating complex emulsified oily wastewater. However, this hybrid system suffers from membrane fouling and subsequent radical quenching. Herein, we overcome these challenges by developing a novel hierarchical filtration-catalysis ceramic membrane to achieve efficient gradient decontamination. This membrane comprises a top hydrophilic MWCNT layer deposited on a CuFe2O4-immobilized ceramic membrane to construct CCuFeCM. A pristine ceramic membrane (CM) and a CuFe2O4-immobilized membrane (CuFeCM) served as controls. Our results demonstrated that CCuFeCM presents the most alleviated fouling potential (∼18% of flux decline) and TOC removal (91%) when treating synthetic textile wastewater containing a mineral oil-in-water emulsion with RhB. Besides that, CCuFeCM achieves the highest PMS-based RhB degradation capability (100%) and initial reaction rate (0.684 min–1). Quenching experiments and EPR analyses show that SO4–•, •OH, and 1O2 are responsible for the CCuFeCM/PMS oxidation system, and 1O2 is the dominant reactive species. The synergistic effect of oil separation and catalytic decomposition is mainly ascribed to the ordered arrangement of selective separation in advance to avoid interference with subsequent AOPs, which allows for micropollutants that are transmitted into internal membrane channels for confined catalytic oxidation. Furthermore, replication filtration tests indicate that CCuFeCM shows durable stable degradation and antifouling performance after simple cleaning. The specific functionality of oil isolation, catalyst anchor, and mass transfer effect reaction compartmentation provides a novel strategy for efficient gradient removal of multiple pollutants in water, which highlights promising application potential under realistic conditions.
研究领域:
环境工程
·
废水处理
·
催化
·
膜技术
·
高级氧化过程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiaxin Li,Huiyu Yi,Yang Xiao,Chenge Liang,Yi Shen,Yungui Li,Qile Fang
Membrane catalysis is a frontier technology for effectively removing organic containments, and burgeoning membranes assembled from two-dimensional (2D) materials have significantly flourished in peroxymonosulfate (PMS)-based catalytic membrane processes. Here, a bottom-up strategy based on restricting CoFe Prussian blue analog (PBA) crystal growth in one direction is used to fabricate large-scale 2D blade-shaped PBA sheets, whose radial size and thickness can be adjusted by the precursor ion ratio (Co II /Fe II ). The stripe CoFe PBA sheets can directly serve as building blocks and are simply assembled into a free-standing 2D membrane by interweaving assembly. The assembled CoFe PBA catalytic membrane possesses excellent wetting properties, guaranteeing an unimpeded mass transfer process, which leads to a superior instantaneous catalytic performance for the antibiotic norfloxacin during the continuous and flow-through membrane catalytic process. SO 4 •− and 1 O 2 are demonstrated to be the main active species, which synergistically contribute to the PMS-driven organic degradation.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Weixuan Guo,Sixiang Zhuang,Ying Peng,Yi Shen,Yungui Li,Suorong Zhang,Qile Fang
Designing high-performance heterostructure catalysts for peroxymonosulfate (PMS) activation is a promising research area. PMS-driven organic pollutant degradation via radical pathways usually suffers from the interference of other coexisting matters. In this study, we took a source design approach and employed a self-templating strategy using Prussian blue analog (PBA) precursors to fabricate CoFe/C heterostructure catalysts dominated by a nonradical pathway. Slow-speed coordination renders the CoFe PBA precursor with a highly ordered crystal structure and fewer coordinated water, resulting in an ideal carbon-encapsulated CoFe bimetallic catalyst (CoFe-S-T) with more high-valence metals and a graphitized carbon layer in its heterostructure; the obtained catalyst is proven to have superior catalytic performance for tetracycline (TC) degradation through a nonradical pathway in PMS-driven oxidation . The high Co III /Co II ratio and surface oxygen content make CoFe-S-T an excellent catalyst by boosting the generation of 1 O 2 , which is the predominant active species. In addition, CoFe-S-T has a high proportion of graphitized carbon layers, which significantly improves the direct electron transfer pathway. Thus, utilizing precursor design in a self-templating strategy is an effective method to synthesize high-performance heterostructures for PMS-driven organic pollutant degradation.
研究领域:
环境科学
·
材料科学
·
化学工程
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Advanced Healthcare Materials
·
2025
·
IF 9.6
Guoqing Cui,Ziyao Lu,Jiangnan Shi,Xinyu He,Yuwei Wang,Hui Chen,Zixiang Jia,Junchang Chen,Jie Han,Hui He,Zhengqing Guo
Overcoming resistance to radiotherapy remains a significant challenge in breast cancer management. A one-step coordinated synthesis of BODIPY -integrated photodynamic nanozymes ( FZBNPs ) that facilitate an orthogonal catalytic cascade for radiotherapy potentiation is presented. The engineered FZBNPs simultaneously alleviate tumor hypoxia through catalase-mimetic oxygen (O 2 ) generation and amplify reactive oxygen species (ROS) production via peroxidase-like activity, synergizing with BODIPY -mediated singlet oxygen ( 1 O 2 ) generation under 660 nm light irradiation. Crucially, FZBNPs deplete intracellular glutathione (GSH) and trigger ferroptosis through lipid peroxidation (LPO) accumulation, directly countering radiotherapy resistance. In vivo validation revealed that the FZBNPs -driven multi-enzymatic cascades achieved near-complete tumor ablation in breast cancer models during radiotherapy. This work establishes a therapeutic paradigm that integrates oxygen modulation, ROS amplification, redox homeostasis disruption, and ferroptosis induction, offering a conceptual basis for the application of enzyme-mimetic nanoplatforms in precision radiation oncology.
研究领域:
纳米医学
·
放射肿瘤学
·
癌症治疗
·
酶模拟
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光动力治疗
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活性氧生物学
·
铁死亡研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Rongwei Zhong,Hu Li,Yangyang Wang,Ying Zhang,Jian Zhou,Tiecheng Wang
Municipal wastewater treatment plants (MWTP) are the main gathering places for antibiotic resistance genes (ARGs) and pathogenic bacteria. In this study, plasma oxidation was applied to remove the ARGs and inhibit pathogenicity in the effluent. The experimental results demonstrated that approximately 1.32 log, 1.34 log, 2.39 log, and 2.80 log of aac (3)-II , bla TEM-1 , Tet W, and Tet C were removed within 25 min of the plasma treatment, respectively. OH, 1 O 2 , O 3 , H 2 O 2 , NO 2 − , and NO 3 − all contributed to ARG removal. Coexisting dissolved organic matter was also oxidized, which was positively related to ARG removal. Plasma oxidation led to a decrease in the diversity and richness of microbial communities; Parcubacteria and Proteobacteria were the main potential hosts of ARGs and mobile genetic elements. Integron gene IntI 1 decreased by 2.46 log after plasma treatment, which was positively related to ARG removal. Gene expression related to ATP binding, DNA repair, gene transfer, and the cell membrane was reduced after plasma treatment, resulting in effective ARG removal. Furthermore, pathogenic genes related to lumpy skin disease, Niemann-Pick disease, polycystic kidney and hepatic disease were all down-regulated by plasma treatment. Overall, the plasma treatment inhibited the transmission risks of ARGs and pathogenicity in the effluent of MWTP.
研究领域:
环境科学
·
微生物学
·
水处理
·
生物技术
✓ 已验证
DOI
高影响因子
Theranostics
·
2021
·
IF 11.556
Wei Qiu,Mengyun Liang,Yuan Gao,Xuelian Yang,Xingyao Zhang,Xiaoli Zhang,Peng Xue,Yuejun Kang,Zhigang Xu
Background: Monotherapy for cancer treatment is limited by unstable efficacy and uncontrollable toxic side effects, while the multifunctional nanoplatform with complex preparation process cannot avoid the potential toxicity of each functional component. Methods: We exploited tumor-specific activated polyamino acid calcified nanoparticles (CHC NPs) as new-type oxidative stress amplification of anticancer drugs via building a safe and biodegradable multifunctional nanoplatform. Giving priority to chemotherapy, and synergizing chemodynamic therapy (CDT) with photodynamic therapy (PDT), this strategy was to achieve enhanced chemotherapy, simultaneously inducing immunogenic cell death and inhibiting tumor cell invasion. Results: Based on amorphous calcium carbonate, pH-responsive nanocarrier was prepared with classical chemotherapeutic drug 10-hydroxycamplothecin (HCPT) and photosensitizer Chlorin e6 (Ce6) to realize multifunctional nanotheranostics. Conclusion: Inventive calcified nanohybrids, where topoisomerase inhibited by HCPT to prevent DNA synthesis, the generation of •OH induced via Fenton reaction, along with a large amount of 1 O 2 produced by Ce6, might be a promising strategy for anti-tumor combination therapy in clinical translation.
研究领域:
纳米技术
·
癌症治疗
·
药学
·
生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaxi Zhang,Fen Wei,Sicen Wang
4-nitrophenol (4-NP) and 2,4-dichlorophenol (2,4-DCP) contaminated wastewater have attracted attention for their genotoxic and carcinogenic hazards. The magnetic MIL-101/CFO was constructed by synergistically integrating porous/hydrophilic/π-conjugated MIL-101(Cr) and CoFe 2 O 4 . The nanocomposites markedly accelerated the catalytic reaction activity. The BET characterizations reveal the nanocomposites had a larger specific surface area and pore volume in comparison to the individual CoFe 2 O 4 . The composite was employed to evaluate the adsorption and peroxymonosulfate (PMS)-activated ability of 4-NP and 2,4-DCP elimination. The adsorption equilibrium could be achieved within 60 min, following the pseudo-second-order kinetic model and the Langmuir isotherm model. The nanocomposites (0.2 g·L −1 ) achieved exceeding 96 % decomposition efficiencies toward 4-NP and 2,4-DCP (0.1 g·L −1 ) after 15 min by PMS (5.29 mM) activation. Notably, the reaction system displayed effective catalytic performance across pH 5 − 11 and resistance to the existence of saline ions and humic acid. According to the free radical quenching experiments and electron paramagnetic resonance, the non-radical route dominant by 1 O 2 and few HO • and SO 4 •− were affirmed to participate the reaction. The recyclable MIL-101/CFO/PMS system approached high adsorption and catalysis ability for phenolics remediation in the environmental application.
研究领域:
环境科学
·
化学工程
·
材料科学
·
水处理
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）